Electron-vibration interaction in the presence of a switchable Kondo resonance realized in a molecular junction.

The interaction of individual electrons with vibrations has been extensively studied. However, the nature of electron-vibration interaction in the presence of many-body electron correlations such as a Kondo state has not been fully investigated. Here, we present transport measurements on a Copper-phthalocyanine molecule, suspended between two silver electrodes in a break-junction setup. Our measurements reveal both zero bias and satellite conductance peaks, which are identified as Kondo resonances with a similar Kondo temperature. The relation of the satellite peaks to electron-vibration interaction is corroborated using several independent spectroscopic indications, as well as ab initio calculations. Further analysis reveals that the contribution of vibration-induced inelastic current is significant in the presence of a Kondo resonance.

Transport properties of individual C60-molecules.

Electrical and thermal transport properties of C60 molecules are investigated with density-functional-theory based calculations. These calculations suggest that the optimum contact geometry for an electrode terminated with a single-Au atom is through binding to one or two C-atoms of C60 with a tendency to promote the sp(2)-hybridization into an sp(3)-type one. Transport in these junctions is primarily through an unoccupied molecular orbital that is partly hybridized with the Au, which results in splitting the degeneracy of the lowest unoccupied molecular orbital triplet. The transmission through these junctions, however, cannot be modeled by a single Lorentzian resonance, as our results show evidence of quantum interference between an occupied and an unoccupied orbital. The interference results in a suppression of conductance around the Fermi energy. Our numerical findings are readily analyzed analytically within a simple two-level model.

Electrochemical gate-controlled electron transport of redox-active single perylene bisimide molecular junctions.

We report a scanning tunneling microscopy (STM) experiment in an electrochemical environment which studies a prototype molecular switch. The target molecules were perylene tetracarboxylic acid bisimides modified with pyridine (P-PBI) and methylthiol (T-PBI) linker groups and with bulky tert-butyl-phenoxy substituents in the bay area. At a fixed bias voltage, we can control the transport current through a symmetric molecular wire Au|P-PBI(T-PBI)|Au by variation of the electrochemical 'gate' potential. The current increases by up to two orders of magnitude. The conductances of the P-PBI junctions are typically a factor 3 larger than those of T-PBI. A theoretical analysis explains this effect as a consequence of shifting the lowest unoccupied perylene level (LUMO) in or out of the bias window when tuning the electrochemical gate potential VG. The difference in on/off ratios reflects the variation of hybridization of the LUMO with the electrode states with the anchor groups. I(T)-E(S(T)) curves of asymmetric molecular junctions formed between a bare Au STM tip and a T-PBI (P-PBI) modified Au(111) electrode in an aqueous electrolyte exhibit a pronounced maximum in the tunneling current at -0.740, which is close to the formal potential of the surface-confined molecules. The experimental data were explained by a sequential two-step electron transfer process.

Nonintegrability of two problems in vortex dynamics.

An analysis is presented of two problems in vortex dynamics whose equations can be written in the Hamiltonian form. They are: the interaction of three coaxial vortex rings and the motion of four point vortices on a sphere. The nonintegrability of these problems in the restricted formulation is demonstrated analytically by the method of split separatrices, using a small parameter. (c) 1997 American Institute of Physics.